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Self-assembled nanostructures in ionic liquids facilitate charge storage at electrified interfaces
Mao, Xianwen Brown, Paul Cervinka, Citrad Hazell, Gavin Li, Hua Ren, Yinying Chen, Di Atkin, Rob Eastoe, Julian Grillo, Isabelle
Mao, Xianwen
Brown, Paul
Cervinka, Citrad
Hazell, Gavin
Li, Hua
Ren, Yinying
Chen, Di
Atkin, Rob
Eastoe, Julian
Grillo, Isabelle
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Publication Date
2019-08-12
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Abstract
Driven by the potential applications of ionic liquids (ILs) in many emerging electrochemical technologies, recent research efforts have been directed at understanding the complex ion ordering in these systems, to uncover novel energy storage mechanisms at IL–electrode interfaces. Here, we discover that surface-active ILs (SAILs), which contain amphiphilic structures inducing self-assembly, exhibit enhanced charge storage performance at electrified surfaces. Unlike conventional non amphiphilic ILs, for which ion distribution is dominated by Coulombic interactions, SAILs exhibit significant and competing van der Waals interactions owing to the non-polar surfactant tails, leading to unusual interfacial ion distributions. We reveal that, at an intermediate degree of electrode polarization, SAILs display optimum performance, because the low-charge-density alkyl tails are effectively excluded from the electrode surfaces, whereas the formation of non-polar domains along the surface suppresses undesired overscreening effects. This work represents a crucial step towards understanding the unique interfacial behaviour and electrochemical properties of amphiphilic liquid systems showing long-range ordering, and offers insights into the design principles for high-energy-density electrolytes based on spontaneous self-assembly behaviour.
Citation
Mao, X., Brown, P., Cervinka, C., Hazell, G., Li, H., Ren, Y., Chen, D., Atkin, R., Eastoe, J., Grillo, I., Padua, A. A. H., Gomes, M. F. C. & Hatton, T. A. (2019). Self-assembled nanostructures in ionic liquids facilitate charge storage at electrified interfaces. Nature Materials, 18, 1350–1357. https://doi.org/10.1038/s41563-019-0449-6
Publisher
Nature Research
Journal
Nature Materials
Research Unit
DOI
10.1038/s41563-019-0449-6
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PubMed Central ID
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Article
Language
en
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ISSN
1476-1122
EISSN
1476-4660